CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improv...CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improvement of device performance.Traditional in-situ ligand replacement and ligand exchange after synthesis were often difficult to control.Here,we proposed a new ligand exchange strategy using a proton-prompted insitu exchange of short 5-aminopentanoic acid ligands with long-chain oleic acid and oleylamine ligands to obtain stable small-size CsPbI_(3)QDs.This exchange strategy maintained the size and morphology of CsPbI_(3)QDs and improved the optical properties and the conductivity of CsPbI_(3)QDs films.As a result,high-efficiency red QD-based light-emitting diodes with an emission wavelength of 645 nm demonstrated a record maximum external quantum efficiency of 24.45%and an operational half-life of 10.79 h.展开更多
BACKGROUND Bevacizumab,an anti-vascular endothelial growth factor(VEGF)monoclonal antibody,inhibits angiogenesis and reduces tumor growth.Serum VEGF-C,lactate dehydrogenase,and inflammatory markers have been reported ...BACKGROUND Bevacizumab,an anti-vascular endothelial growth factor(VEGF)monoclonal antibody,inhibits angiogenesis and reduces tumor growth.Serum VEGF-C,lactate dehydrogenase,and inflammatory markers have been reported as predictive markers related to bevacizumab treatment.Programmed cell death ligand 1(PD-L1)could act upon VEGF receptor 2 to induce cancer cell angiogenesis and metastasis.AIM To investigate the efficacy of bevacizumab-containing chemotherapy in patients with metastatic colorectal cancer(CRC)according to the expression of PD-L1.METHODS This analysis included CRC patients who received bevacizumab plus FOLFOX or FOLFIRI as first-line therapy between June 24,2014 and February 28,2022,at Samsung Medical Center(Seoul,South Korea).Analysis of patient data included evaluation of PD-L1 expression by the combined positive score(CPS).We analyzed the efficacy of bevacizumab according to PD-L1 expression status in patients with CRC.RESULTS A total of 124 patients was included in this analysis.Almost all patients were treated with bevacizumab plus FOLFIRI or FOLFOX as the first-line chemotherapy.While 77%of patients received FOLFOX,23%received FOLFIRI as backbone first-line chemotherapy.The numbers of patients with a PD-L1 CPS of 1 or more,5 or more,or 10 or more were 105(85%),64(52%),and 32(26%),respectively.The results showed no significant difference in progression-free survival(PFS)and overall survival(OS)with bevacizumab treatment between patients with PDL1 CPS less than 1 and those with PD-L1 CPS of 1 or more(PD-L1<1%vs PD-L1≥1%;PFS:P=0.93,OS:P=0.33),between patients with PD-L1 CPS less than 5 and of 5 or more(PD-L1<5%vs PD-L1≥5%;PFS:P=0.409,OS:P=0.746),and between patients with PD-L1 CPS less than 10 and of 10 or more(PD-L1<10%vs PD-L1≥10%;PFS:P=0.529,OS:P=0.568).CONCLUSION Chemotherapy containing bevacizumab can be considered as first-line therapy in metastatic CRC irrespective of PD-L1 expression.展开更多
Remarkable progress has characterized the field of electrocatalysis in recent decades,driven in part by an enhanced comprehension of catalyst structures and mechanisms at the nanoscale.Atomically precise metal nanoclu...Remarkable progress has characterized the field of electrocatalysis in recent decades,driven in part by an enhanced comprehension of catalyst structures and mechanisms at the nanoscale.Atomically precise metal nanoclusters,serving as exemplary models,significantly expand the range of accessible structures through diverse cores and ligands,creating an exceptional platform for the investigation of catalytic reactions.Notably,ligand‐protected Au nanoclusters(NCs)with precisely defined core numbers offer a distinct advantage in elucidating the correlation between their specific structures and the reaction mechanisms in electrocatalysis.The strategic modulation of the fine microstructures of Au NCs presents crucial opportunities for tailoring their electrocatalytic performance across various reactions.This review delves into the profound structural effects of Au NC cores and ligands in electrocatalysis,elucidating their underlying mechanisms.A detailed exploration of the fundamentals of Au NCs,considering core and ligand structures,follows.Subsequently,the interaction between the core and ligand structures of Au NCs and their impact on electrocatalytic performance in diverse reactions are examined.Concluding the discourse,challenges and personal prospects are presented to guide the rational design of efficient electrocatalysts and advance electrocatalytic reactions.展开更多
Under solvothermal conditions,six new coordination polymers(CPs)[Mn(L)(phen)(H_(2)O)]_(n)(1),[Co(L)(phen)(H_(2)O)]_(n)(2),[Cu(L)(phen)(H_(2)O)]_(n)(3),[Zn_(2)(L)_(2)(phen)2(H_(2)O)]_(n)(4),[Zn(L)(phen)]_(n)(5),and[Cd(...Under solvothermal conditions,six new coordination polymers(CPs)[Mn(L)(phen)(H_(2)O)]_(n)(1),[Co(L)(phen)(H_(2)O)]_(n)(2),[Cu(L)(phen)(H_(2)O)]_(n)(3),[Zn_(2)(L)_(2)(phen)2(H_(2)O)]_(n)(4),[Zn(L)(phen)]_(n)(5),and[Cd(L)(phen)2]_(n)(6)were synthesized by reactions of dicarboxylate ligand 2,2'-(1,2-phenylenebis(methylene))bis(sulfanediyl)dinobutyric acid(H_(2)L)and 1,10-phenanthroline(phen)with the corresponding metal salts.Complexes 1-6 have been structurally characterized by single-crystal X-ray diffraction analyses,elemental analysis,IR,thermogravimetric analysis,and powder X-ray diffraction.The structures of 1-6 are 1D chains,which are further connected by hydrogen bonding interac-tions to form 3D supramolecular structures.Among them,1 and 2 are isomorphic with L2-of syn-conformation,while L2-shows anti-conformation in 3-6.In addition,the solid-state photoluminescence property of 4-6 was investigated.展开更多
Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand ...Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand impedes the adsorption and activation of CO_(2)molecules in practical applications.Here,a ligand modulation technology is employed to enhance the photocatalytic CO_(2)reduction activity of lead-free Cs_(2)AgInCl_(6)microcrystals(MCs).The Cs_(2)AgInCl_(6)MCs passivated by Oleic acid(OLA)and Octanoic acid(OCA)are used for photocatalytic CO_(2)reduction.The results show that the surface defects and electronic properties of Cs_(2)AgInCl_(6)MCs can be adjusted through ligand modulation.Compared with the OLA-Cs_(2)AgInCl_(6),the OCA-Cs_(2)AgInCl_(6)catalyst demonstrated a significant improvement in the catalytic yield of CO and CH_(4).The CO and CH_(4)catalytic yields of OCA-Cs_(2)AgInCl_(6)reached 171.88 and34.15μmol g^(-1)h^(-1)which were 2.03 and 12.98 times higher than those of OLA-Cs_(2)AgInCl_(6),and the total electron consumption rate of OCA-Cs_(2)AgInCl_(6)was 615.2μmol g^(-1)h^(-1)which was 3.25 times higher than that of OLA-Cs_(2)AgInCl_(6).Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs_(2)AgInCl_(6)MCs induced by ligand modulation.This study illustrates the potential of lead-free Cs_(2)AgInCl_(6)MCs for efficient photocatalytic CO_(2)reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.展开更多
BACKGROUND Anti-programmed death-1/programmed death-ligand 1(PD-1/PD-L1)immuno-therapy has demonstrated promising results on gastric cancer(GC).However,PD-L1 can express differently between metastatic sites and primar...BACKGROUND Anti-programmed death-1/programmed death-ligand 1(PD-1/PD-L1)immuno-therapy has demonstrated promising results on gastric cancer(GC).However,PD-L1 can express differently between metastatic sites and primary tumors(PT).AIM To compare PD-L1 status in PT and matched lymph node metastases(LNM)of GC patients and to determine the correlation between the PD-L1 status and clinicopathological characteristics.METHODS We retrospectively reviewed 284 GC patients who underwent D2-gastrectomy.PD-L1 was evaluated by immunohistochemistry(clone SP142)using the com-bined positive score.All PD-L1+PT staged as pN+were also tested for PD-L1 expression in their LNM.PD-L1(-)GC with pN+served as the comparison group.RESULTS Among 284 GC patients included,45 had PD-L1+PT and 24 of them had pN+.For comparison,44 PD-L1(-)cases with pN+were included(sample loss of 4 cases).Of the PD-L1+PT,54.2%(13/24 cases)were also PD-L1+in the LNM.Regarding PD-L1(-)PT,9.1%(4/44)had PD-L1+in the LNM.The agreement between PT and LNM had a kappa value of 0.483.Larger tumor size and moderate/severe peritumoral inflammatory response were associated with PD-L1 positivity in both sites.There was no statistical difference in overall survival for PT and LNM according to the PD-L1 status(P=0.166 and P=0.837,respectively).CONCLUSION Intra-patient heterogeneity in PD-L1 expression was observed between the PT and matched LNM.This disagreement in PD-L1 status may emphasize the importance of considering different tumor sites for analyses to select patients for immunotherapy.展开更多
Spinal cord injury involves non-reversible damage to the central nervous system that is characterized by limited regenerative capacity and secondary inflammatory damage.The expression of the C-C motif chemokine ligand...Spinal cord injury involves non-reversible damage to the central nervous system that is characterized by limited regenerative capacity and secondary inflammatory damage.The expression of the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis exhibits significant differences before and after injury.Recent studies have revealed that the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis is closely associated with secondary inflammatory responses and the recruitment of immune cells following spinal cord injury,suggesting that this axis is a novel target and regulatory control point for treatment.This review comprehensively examines the therapeutic strategies targeting the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis,along with the regenerative and repair mechanisms linking the axis to spinal cord injury.Additionally,we summarize the upstream and downstream inflammatory signaling pathways associated with spinal cord injury and the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis.This review primarily elaborates on therapeutic strategies that target the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis and the latest progress of research on antagonistic drugs,along with the approaches used to exploit new therapeutic targets within the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis and the development of targeted drugs.Nevertheless,there are presently no clinical studies relating to spinal cord injury that are focusing on the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis.This review aims to provide new ideas and therapeutic strategies for the future treatment of spinal cord injury.展开更多
Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,...Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,phen=phenanthroline,bpe=1,2⁃bis(4⁃pyridyl)ethylene)were synthesized by solvothermal reactions and characterized by single⁃crystal X⁃ray diffraction,thermogravimetric analyses,IR spectroscopy and elemental analysis.1 displays a 1D chain struc⁃ture,and these chains are joined by O-H…O hydrogen bonding andπ⁃πstacking interactions to generate a 2D layer structure.2 displays a 2D layer structure,and adjacent layers are generated 3D architecture throughπ⁃πstacking interactions.3 displays a 1D chain structure,and adjacent chains are generated double layer structure through O-H…O hydrogen bonding.The fluorescent properties of 1 and 3 indicate that they can potentially be used as a luminescent sensor.1 was highly selective and sensitive towards o⁃nitrophenol through different detection mechanisms,however,3 was highly selective and sensitive towards 2,4,6⁃trinitrophenol.In addition,the magnetic behavior of 2 has also been investigated.CCDC:2172533,1,2355773,2,2355774,3.展开更多
Heavy metal contaminated water sources pose serious health risks for humans,animals,and plants.Exposure to and ingestion of heavy metals have been associated to liver,kidney,and brain function.Objective:The aim of thi...Heavy metal contaminated water sources pose serious health risks for humans,animals,and plants.Exposure to and ingestion of heavy metals have been associated to liver,kidney,and brain function.Objective:The aim of this research is to comparatively examine the metal removal efficacy of three solid bidentate chemicals and four plant materials.Study Design&Methods:Standard solutions of zinc(II)and lead(II)ions with concentrations of 1,000 ppm were respectively treated with OA(Oxalic Acid),dibasic bidentate ligands(sodium hydrogen phosphate and sodium carbonate).Then,the solutions were placed on a shaker for 15 h,centrifuged,and the supernatant was analyzed using ICP-AES(Inductively Coupled Plasma-Atomic Emission Spectrometry).Results:All the solid bidentate adsorbents were very effective in removing zinc and lead(>90%).However,more lead than zinc was removed across all adsorbents except for lemon where equal percent of zinc and lead(49%)were removed.OA and Na2HPO4 removed about equal amount of lead(>99%).The plant materials(SP(Spinach),bell pepper and GBP(Green Bell Pepper)),respectively and preferentially removed more lead(98.9%,98.3%,81.5%)than zinc(91.7%,46%,46%).Conclusion:Although plant materials have gained attraction for the remediation of heavy metal,however,some bidentate chemical ligands such as OA,sodium carbonate and sodium hydrogen phosphates are even more effective in removing these metals from contaminated water.Furthermore,heavier metals are preferentially removed than lighter metals.展开更多
Oriented ligand immobilization is one of the most effective strategies used in the design and construction of a high-capacity protein A chromatography. In this work, cysteine was introduced as anchoring sites by subst...Oriented ligand immobilization is one of the most effective strategies used in the design and construction of a high-capacity protein A chromatography. In this work, cysteine was introduced as anchoring sites by substituting a specific residue on Helix Ⅰ, Ⅱ, and at C-terminus of antibody binding domain Z from protein A, respectively, to investigate structural evolution and binding behavior of protein A ligands at liquid-solid interfaces. Among the three affinity dextran-coated Fe_(3)O_(4) magnetic nanoparticles(Fe_(3)O_(4)@Dx MNPs), affinity MNPs with the immobilized ligand via N11C on Helix Ⅰ(Fe_(3)O_(4)@Dx-Z_(1) MNPs) had the highest helical content, and MNPs with the immobilized ligand via G29C on Helix Ⅱ(Fe_(3)O_(4)@Dx-Z_(2) MNPs) had the lowest helical content at the same pHs. It was attributed to less electrostatic attraction of ligand to negatively charged surface on Fe_(3)O_(4)@Dx-Z_(1) MNPs because of less positive charged residues on Helix Ⅰ(K6) than Helix Ⅱ(R27/K35). Among the three affinity MNPs, moreover, the highest affinity to immunoglobulin G(IgG) binding was observed on Fe_(3)O_(4)@Dx-Z_(1) MNPs in isothermal titration calorimetry measurement, further validating greater structural integrity of the ligand on Fe_(3)O_(4)@Dx-Z_(1) MNPs. Finally,the study of IgG binding on MNPs and 96-well plates showed that anchoring sites for ligand immobilization had distinct influences on IgG binding and IgG-mediated antigen binding. This work illustrated that anchoring sites of the ligands had a striking significance for the molecular structure of the ligand at liquid-solid interfaces and raised an important implication for the design and optimization of protein A chromatography and protein A-based immunoassay analysis.展开更多
Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,t...Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported[Au_(25)(PET)_(18)]-nanoclusters with the preservation of the core structure.This procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment,avoiding the reconfiguration or agglomeration of Au_(25)nanoclusters,where the degree of dethiolation can be regulated by the control of duration.This work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution reaction.Consequently,the activity and selectivity towards CO formation in electrochemical CO_(2)reduction reaction of Au_(25)nanoclusters can be promoted.This work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.展开更多
The design of efficient and robust non-precious metal electrocatalysts towards oxygen evolution reaction(OER)is of great value for developing green energy technologies.The in-situ formed high-valence(oxy)hydroxides sp...The design of efficient and robust non-precious metal electrocatalysts towards oxygen evolution reaction(OER)is of great value for developing green energy technologies.The in-situ formed high-valence(oxy)hydroxides species during the reconstruction process of pre-catalysts are recognized as the real contributing sites for OER.However,pre-catalysts generally undergo a slow and inadequate self-reconstruction.Herein,we reported a PO^(3-)_(4)optimized CoFe-based OER catalysts with amorphous structure,which enables a fast and deep reconstruction during the OER process.The amorphous structure induced by ligands PO^(3-)_(4)is prone to evolution and further form active species for OER.The electron interaction between metal sites can be modulated by electron-rich PO^(3-)_(4),which promotes generation of high active CoOOH.Simultaneously,the etching of PO^(3-)_(4)from the pre-catalysts during the catalytic process is in favor of accelerating the self-reconstruction.As a result,as-prepared precatalyst can generate high active CoOOH at a low potential of 1.4 V and achieve an in-depth reconstructed nanosheet structure with abundant OER active sites.Our work provides a promising design of pre-catalysts for realizing efficient catalysis of water oxidation.展开更多
Deep-level defects and random oriented configuration in perovskite crystallization process would cause the nonradiative recombination and further affect the performance of perovskite solar cells(PSCs).Herein,two metal...Deep-level defects and random oriented configuration in perovskite crystallization process would cause the nonradiative recombination and further affect the performance of perovskite solar cells(PSCs).Herein,two metal-organic frameworks(MOFs)with tunable Lewis-base passivation sites have been constructed(Cd-Httb and Cd-Httb-BDC,Httb=5-(4-(1H-1,2,4-triazole-1-yl)benzyl)-1h-tetrazole,BDC=1,4-dicarboxybenzene)to eliminate deep-level defects and simultaneously as nanostructured heterogeneous nucleation seed to assist the growth of large-grained perovskite films.Compared with the control and Cd-Httb,Cd-Httb-BDC designed with mix-ligands strategy exhibited the enhanced inducted effect on the crystallization and nucleation of high-quality perovskite films during annealing process.Consequently,the resultant Cd-Httb-BDC-modified device achieved higher power conversion efficiency(PCE)(22.18%)than the control(20.89%)and Cd-Httb(21.56%).Meanwhile,the unencapsulated Cd-Httb-BDC-modified device still maintained 90%of initial PCE after 1500 h in ambient conditions and exhibited enhanced thermal stability(85℃ in N_(2) atmosphere).This work presented a successful example of mixligands strategy on construction of high-quality MOF-assisted perovskite films for high-efficient and stable PSCs.展开更多
Cancer is one of the most prevalent diseases worldwide,which causes significant morbidity and mortality.Designing and developing a potential anti-cancer drug is an active field of research worldwide.Microorganisms hav...Cancer is one of the most prevalent diseases worldwide,which causes significant morbidity and mortality.Designing and developing a potential anti-cancer drug is an active field of research worldwide.Microorganisms have been considered a potential source of anti-cancer drugs.One such microbe-derived compound is surfactin,which shows potential anti-cancer activities.In this study,we evaluated the binding potential of surfactin with several cancer cell ligands via an in-silico approach.Hence,molecular docking studies were performed to test the binding potential of surfactin against four targets.The analyses revealed that surfactin from Bacillus sp.can bind with the targeted ligands(coenzyme A,D-leucine,glycerol,and(R)-3-hydroxytetradecanal)with significant affinity.Surfactin showed the highest binding affinity(-7.7 kcal mol-1)to coenzyme A among the targeted ligands.These results may be useful for developing anti-cancer drugs.Nevertheless,further experimental studies are needed to investigate the ligand binding capacity and anti-cancer potential of such surfactin-like molecules.展开更多
Bimetallic nanoparticles exhibit a synergistic effect that critically depends on their surface composition,but such promotion mechanisms become vague with varying surface compositions.Here,alumina supported Ag@Pd core...Bimetallic nanoparticles exhibit a synergistic effect that critically depends on their surface composition,but such promotion mechanisms become vague with varying surface compositions.Here,alumina supported Ag@Pd core–shell and PdAg alloy structure with controlled size and surface compositions were prepared to demonstrate synergetic mechanisms,particularly,ligand and strain effects on activity and ethylene selectivity for acetylene hydrogenation.The performance evaluation indicates that Ag@Pd catalysts with well-controlled Pd-shell thickness can effectively lower apparent activation energy and improve ethylene selectivity.Hydrogenation activity increases from 0.019 to 0.062 s^(-1) with decreasing Pd-shell thickness under mild conditions,which is 3–6 times higher than their alloyed and monometallic counterparts.Combined characterizations and density functional theory are conducted to reveal such shell-thickness-dependent performance.The ligand effect arising from Ag alloying in the interface of Ag@Pd2ML observes the strongest binding of acetylene,but it diminished sharply and the strain effect gets more prevailing with increasing shell thickness.The competition of ethylene desorption and deephydrogenation were also investigated to understand the selectivity governing factors,and the selectivity descriptor(0.5BE(C_(2)H_(4))–BE(H))was built to match the contribution of ligand and strain effect on the different surfaces of Pd-Ag bimetallic NPs.The exploration of synergetic mechanisms among bimetallic NPs with varied structure and surface compositions in this work can help us to deepen the understanding catalyst structure–activity relationship and provide a feasible way to optimize the overall catalytic performance.展开更多
Perovskite solar cells(PSCs)have attracted aggressive attention in the photovoltaic field in light of the rapid increasing power conversion efficiency.However,their large-scale application and commercialization are li...Perovskite solar cells(PSCs)have attracted aggressive attention in the photovoltaic field in light of the rapid increasing power conversion efficiency.However,their large-scale application and commercialization are limited by the toxicity issue of lead(Pb).Among all the lead-free perovskites,tin(Sn)-based perovskites have shown potential due to their low toxicity,ideal bandgap structure,high carrier mobility,and long hot carrier lifetime.Great progress of Sn-based PSCs has been realized in recent years,and the certified efficiency has now reached over 14%.Nevertheless,this record still falls far behind the theoretical calculations.This is likely due to the uncontrolled nucleation states and pronounced Sn(Ⅳ)vacancies.With insights into the methodologies resolving both issues,ligand engineering-assisted perovskite film fabrication dictates the state-of-the-art Sn-based PSCs.Herein,we summarize the role of ligand engineering during each state of film fabrication,ranging from the starting precursors to the ending fabricated bulks.The incorporation of ligands to suppress Sn~(2+)oxidation,passivate bulk defects,optimize crystal orientation,and improve stability is discussed,respectively.Finally,the remained challenges and perspectives toward advancing the performance of Sn-based PSCs are presented.We expect this review can draw a clear roadmap to facilitate Sn-based PSCs via ligand engineering.展开更多
The performance of inverted quantum-dot light-emitting diodes(QLEDs)based on solution-processed hole transport layers(HTLs)has been limited by the solvent-induced damage to the quantum dot(QD)layer during the spin-coa...The performance of inverted quantum-dot light-emitting diodes(QLEDs)based on solution-processed hole transport layers(HTLs)has been limited by the solvent-induced damage to the quantum dot(QD)layer during the spin-coating of the HTL.The lack of compatibility between the HTL’s solvent and the QD layer results in an uneven surface,which negatively impacts the overall device performance.In this work,we develop a novel method to solve this problem by modifying the QD film with 1,8-diaminooctane to improve the resistance of the QD layer for the HTL’s solvent.The uniform QD layer leads the inverted red QLED device to achieve a low turn-on voltage of 1.8 V,a high maximum luminance of 105500 cd/m2,and a remarkable maximum external quantum efficiency of 13.34%.This approach releases the considerable potential of HTL materials selection and offers a promising avenue for the development of high-performance inverted QLEDs.展开更多
We previously reported that postsynaptic density-93 mediates neuron-microglia crosstalk by interacting with amino acids 357–395 of C-X3-C motif chemokine ligand 1(CX3 CL1) to induce microglia polarization. More impor...We previously reported that postsynaptic density-93 mediates neuron-microglia crosstalk by interacting with amino acids 357–395 of C-X3-C motif chemokine ligand 1(CX3 CL1) to induce microglia polarization. More importantly, the peptide Tat-CX3 CL1(comprising amino acids 357–395 of CX3 CL1) disrupts the interaction between postsynaptic density-93 and CX3 CL1, reducing neurological impairment and exerting a protective effect in the context of acute ischemic stroke. However, the mechanism underlying these effects remains unclear. In the current study, we found that the pro-inflammatory M1 phenotype increased and the anti-inflammatory M2 phenotype decreased at different time points. The M1 phenotype increased at 6 hours after stroke and peaked at 24 hours after perfusion, whereas the M2 phenotype decreased at 6 and 24 hours following reperfusion. We found that the peptide Tat-CX3 CL1(357–395 aa) facilitates microglial polarization from M1 to M2 by reducing the production of soluble CX3 CL1. Furthermore, the a disintegrin and metalloprotease domain 17(ADAM17) inhibitor GW280264 x, which inhibits metalloprotease activity and prevents CX3 CL1 from being sheared into its soluble form, facilitated microglial polarization from M1 to M2 by inhibiting soluble CX3 CL1 formation. Additionally, Tat-CX3 CL1(357–395 aa) attenuated long-term cognitive deficits and improved white matter integrity as determined by the Morris water maze test at 31–34 days following surgery and immunofluorescence staining at 35 days after stroke, respectively. In conclusion, Tat-CX3 CL1(357–395 aa) facilitates functional recovery after ischemic stroke by promoting microglial polarization from M1 to M2. Therefore, the Tat-CX3 CL1(357–395 aa) is a potential therapeutic agent for ischemic stroke.展开更多
基金This work was financially supported by the National Key Research and Development Program of China(2022YFB3602902)the Key Projects of National Natural Science Foundation of China(62234004)+5 种基金Innovation and Entrepreneurship Team of Zhejiang Province(2021R01003)Science and Technology Innovation 2025 Major Project of Ningbo(2022Z085)Ningbo 3315 Programme(2020A-01-B)YONGJIANG Talent Introduction Programme(2021A-038-B)Flexible Electronics Zhejiang Province Key Laboratory Fund Project(2022FEO02)Zhejiang Provincial Natural Science Foundation of China(LR21F050001).
文摘CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improvement of device performance.Traditional in-situ ligand replacement and ligand exchange after synthesis were often difficult to control.Here,we proposed a new ligand exchange strategy using a proton-prompted insitu exchange of short 5-aminopentanoic acid ligands with long-chain oleic acid and oleylamine ligands to obtain stable small-size CsPbI_(3)QDs.This exchange strategy maintained the size and morphology of CsPbI_(3)QDs and improved the optical properties and the conductivity of CsPbI_(3)QDs films.As a result,high-efficiency red QD-based light-emitting diodes with an emission wavelength of 645 nm demonstrated a record maximum external quantum efficiency of 24.45%and an operational half-life of 10.79 h.
文摘BACKGROUND Bevacizumab,an anti-vascular endothelial growth factor(VEGF)monoclonal antibody,inhibits angiogenesis and reduces tumor growth.Serum VEGF-C,lactate dehydrogenase,and inflammatory markers have been reported as predictive markers related to bevacizumab treatment.Programmed cell death ligand 1(PD-L1)could act upon VEGF receptor 2 to induce cancer cell angiogenesis and metastasis.AIM To investigate the efficacy of bevacizumab-containing chemotherapy in patients with metastatic colorectal cancer(CRC)according to the expression of PD-L1.METHODS This analysis included CRC patients who received bevacizumab plus FOLFOX or FOLFIRI as first-line therapy between June 24,2014 and February 28,2022,at Samsung Medical Center(Seoul,South Korea).Analysis of patient data included evaluation of PD-L1 expression by the combined positive score(CPS).We analyzed the efficacy of bevacizumab according to PD-L1 expression status in patients with CRC.RESULTS A total of 124 patients was included in this analysis.Almost all patients were treated with bevacizumab plus FOLFIRI or FOLFOX as the first-line chemotherapy.While 77%of patients received FOLFOX,23%received FOLFIRI as backbone first-line chemotherapy.The numbers of patients with a PD-L1 CPS of 1 or more,5 or more,or 10 or more were 105(85%),64(52%),and 32(26%),respectively.The results showed no significant difference in progression-free survival(PFS)and overall survival(OS)with bevacizumab treatment between patients with PDL1 CPS less than 1 and those with PD-L1 CPS of 1 or more(PD-L1<1%vs PD-L1≥1%;PFS:P=0.93,OS:P=0.33),between patients with PD-L1 CPS less than 5 and of 5 or more(PD-L1<5%vs PD-L1≥5%;PFS:P=0.409,OS:P=0.746),and between patients with PD-L1 CPS less than 10 and of 10 or more(PD-L1<10%vs PD-L1≥10%;PFS:P=0.529,OS:P=0.568).CONCLUSION Chemotherapy containing bevacizumab can be considered as first-line therapy in metastatic CRC irrespective of PD-L1 expression.
基金Guangzhou Key R&D Program/Plan Unveiled Flagship Project,Grant/Award Number:20220602JBGS02Guangzhou Basic and Applied Basic Research Project,Grant/Award Number:202201011449+3 种基金Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology,Grant/Award Numbers:FC202220,FC202216Guangdong Basic and Applied Basic Research Foundation,Grant/Award Numbers:2021A1515010167,2022A1515011196National Natural Science Foundation of China,Grant/Award Numbers:21975292,21978331,22068008,52101186Training Program of the Major Research Plan of the National Natural Science Foundation of China,Grant/Award Number:92061124。
文摘Remarkable progress has characterized the field of electrocatalysis in recent decades,driven in part by an enhanced comprehension of catalyst structures and mechanisms at the nanoscale.Atomically precise metal nanoclusters,serving as exemplary models,significantly expand the range of accessible structures through diverse cores and ligands,creating an exceptional platform for the investigation of catalytic reactions.Notably,ligand‐protected Au nanoclusters(NCs)with precisely defined core numbers offer a distinct advantage in elucidating the correlation between their specific structures and the reaction mechanisms in electrocatalysis.The strategic modulation of the fine microstructures of Au NCs presents crucial opportunities for tailoring their electrocatalytic performance across various reactions.This review delves into the profound structural effects of Au NC cores and ligands in electrocatalysis,elucidating their underlying mechanisms.A detailed exploration of the fundamentals of Au NCs,considering core and ligand structures,follows.Subsequently,the interaction between the core and ligand structures of Au NCs and their impact on electrocatalytic performance in diverse reactions are examined.Concluding the discourse,challenges and personal prospects are presented to guide the rational design of efficient electrocatalysts and advance electrocatalytic reactions.
文摘Under solvothermal conditions,six new coordination polymers(CPs)[Mn(L)(phen)(H_(2)O)]_(n)(1),[Co(L)(phen)(H_(2)O)]_(n)(2),[Cu(L)(phen)(H_(2)O)]_(n)(3),[Zn_(2)(L)_(2)(phen)2(H_(2)O)]_(n)(4),[Zn(L)(phen)]_(n)(5),and[Cd(L)(phen)2]_(n)(6)were synthesized by reactions of dicarboxylate ligand 2,2'-(1,2-phenylenebis(methylene))bis(sulfanediyl)dinobutyric acid(H_(2)L)and 1,10-phenanthroline(phen)with the corresponding metal salts.Complexes 1-6 have been structurally characterized by single-crystal X-ray diffraction analyses,elemental analysis,IR,thermogravimetric analysis,and powder X-ray diffraction.The structures of 1-6 are 1D chains,which are further connected by hydrogen bonding interac-tions to form 3D supramolecular structures.Among them,1 and 2 are isomorphic with L2-of syn-conformation,while L2-shows anti-conformation in 3-6.In addition,the solid-state photoluminescence property of 4-6 was investigated.
基金the National Natural Science Foundation of China(Grant No.62375032)the Natural Science Foundation of Chongqing(Grant No.CSTB2023TIADKPX0017)+2 种基金the Open Fund of the State Key Laboratory of High Field Laser Physics(Shanghai Institute of Optics and Fine Mechanics)the China Postdoctoral Science Foundation(Grant No.BX20230355)the Department of Education of Guizhou Province(Guizhou Teaching and Technology[2023]015)。
文摘Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand impedes the adsorption and activation of CO_(2)molecules in practical applications.Here,a ligand modulation technology is employed to enhance the photocatalytic CO_(2)reduction activity of lead-free Cs_(2)AgInCl_(6)microcrystals(MCs).The Cs_(2)AgInCl_(6)MCs passivated by Oleic acid(OLA)and Octanoic acid(OCA)are used for photocatalytic CO_(2)reduction.The results show that the surface defects and electronic properties of Cs_(2)AgInCl_(6)MCs can be adjusted through ligand modulation.Compared with the OLA-Cs_(2)AgInCl_(6),the OCA-Cs_(2)AgInCl_(6)catalyst demonstrated a significant improvement in the catalytic yield of CO and CH_(4).The CO and CH_(4)catalytic yields of OCA-Cs_(2)AgInCl_(6)reached 171.88 and34.15μmol g^(-1)h^(-1)which were 2.03 and 12.98 times higher than those of OLA-Cs_(2)AgInCl_(6),and the total electron consumption rate of OCA-Cs_(2)AgInCl_(6)was 615.2μmol g^(-1)h^(-1)which was 3.25 times higher than that of OLA-Cs_(2)AgInCl_(6).Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs_(2)AgInCl_(6)MCs induced by ligand modulation.This study illustrates the potential of lead-free Cs_(2)AgInCl_(6)MCs for efficient photocatalytic CO_(2)reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.
基金The study was approved by the hospital ethics committee and registered online(https://plataformabrasil.saude.gov.br,CAAE:26380019.6.0000.0065).
文摘BACKGROUND Anti-programmed death-1/programmed death-ligand 1(PD-1/PD-L1)immuno-therapy has demonstrated promising results on gastric cancer(GC).However,PD-L1 can express differently between metastatic sites and primary tumors(PT).AIM To compare PD-L1 status in PT and matched lymph node metastases(LNM)of GC patients and to determine the correlation between the PD-L1 status and clinicopathological characteristics.METHODS We retrospectively reviewed 284 GC patients who underwent D2-gastrectomy.PD-L1 was evaluated by immunohistochemistry(clone SP142)using the com-bined positive score.All PD-L1+PT staged as pN+were also tested for PD-L1 expression in their LNM.PD-L1(-)GC with pN+served as the comparison group.RESULTS Among 284 GC patients included,45 had PD-L1+PT and 24 of them had pN+.For comparison,44 PD-L1(-)cases with pN+were included(sample loss of 4 cases).Of the PD-L1+PT,54.2%(13/24 cases)were also PD-L1+in the LNM.Regarding PD-L1(-)PT,9.1%(4/44)had PD-L1+in the LNM.The agreement between PT and LNM had a kappa value of 0.483.Larger tumor size and moderate/severe peritumoral inflammatory response were associated with PD-L1 positivity in both sites.There was no statistical difference in overall survival for PT and LNM according to the PD-L1 status(P=0.166 and P=0.837,respectively).CONCLUSION Intra-patient heterogeneity in PD-L1 expression was observed between the PT and matched LNM.This disagreement in PD-L1 status may emphasize the importance of considering different tumor sites for analyses to select patients for immunotherapy.
基金supported by the National Natural Science Foundation of China(Key Program),No.11932013the National Natural Science Foundation of China(General Program),No.82272255+2 种基金Armed Police Force High-Level Science and Technology Personnel ProjectThe Armed Police Force Focuses on Supporting Scientific and Technological Innovation TeamsKey Project of Tianjin Science and Technology Plan,No.20JCZDJC00570(all to XC)。
文摘Spinal cord injury involves non-reversible damage to the central nervous system that is characterized by limited regenerative capacity and secondary inflammatory damage.The expression of the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis exhibits significant differences before and after injury.Recent studies have revealed that the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis is closely associated with secondary inflammatory responses and the recruitment of immune cells following spinal cord injury,suggesting that this axis is a novel target and regulatory control point for treatment.This review comprehensively examines the therapeutic strategies targeting the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis,along with the regenerative and repair mechanisms linking the axis to spinal cord injury.Additionally,we summarize the upstream and downstream inflammatory signaling pathways associated with spinal cord injury and the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis.This review primarily elaborates on therapeutic strategies that target the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis and the latest progress of research on antagonistic drugs,along with the approaches used to exploit new therapeutic targets within the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis and the development of targeted drugs.Nevertheless,there are presently no clinical studies relating to spinal cord injury that are focusing on the C-C motif chemokine ligand 2/C-C motif chemokine receptor 2 axis.This review aims to provide new ideas and therapeutic strategies for the future treatment of spinal cord injury.
文摘Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,phen=phenanthroline,bpe=1,2⁃bis(4⁃pyridyl)ethylene)were synthesized by solvothermal reactions and characterized by single⁃crystal X⁃ray diffraction,thermogravimetric analyses,IR spectroscopy and elemental analysis.1 displays a 1D chain struc⁃ture,and these chains are joined by O-H…O hydrogen bonding andπ⁃πstacking interactions to generate a 2D layer structure.2 displays a 2D layer structure,and adjacent layers are generated 3D architecture throughπ⁃πstacking interactions.3 displays a 1D chain structure,and adjacent chains are generated double layer structure through O-H…O hydrogen bonding.The fluorescent properties of 1 and 3 indicate that they can potentially be used as a luminescent sensor.1 was highly selective and sensitive towards o⁃nitrophenol through different detection mechanisms,however,3 was highly selective and sensitive towards 2,4,6⁃trinitrophenol.In addition,the magnetic behavior of 2 has also been investigated.CCDC:2172533,1,2355773,2,2355774,3.
文摘Heavy metal contaminated water sources pose serious health risks for humans,animals,and plants.Exposure to and ingestion of heavy metals have been associated to liver,kidney,and brain function.Objective:The aim of this research is to comparatively examine the metal removal efficacy of three solid bidentate chemicals and four plant materials.Study Design&Methods:Standard solutions of zinc(II)and lead(II)ions with concentrations of 1,000 ppm were respectively treated with OA(Oxalic Acid),dibasic bidentate ligands(sodium hydrogen phosphate and sodium carbonate).Then,the solutions were placed on a shaker for 15 h,centrifuged,and the supernatant was analyzed using ICP-AES(Inductively Coupled Plasma-Atomic Emission Spectrometry).Results:All the solid bidentate adsorbents were very effective in removing zinc and lead(>90%).However,more lead than zinc was removed across all adsorbents except for lemon where equal percent of zinc and lead(49%)were removed.OA and Na2HPO4 removed about equal amount of lead(>99%).The plant materials(SP(Spinach),bell pepper and GBP(Green Bell Pepper)),respectively and preferentially removed more lead(98.9%,98.3%,81.5%)than zinc(91.7%,46%,46%).Conclusion:Although plant materials have gained attraction for the remediation of heavy metal,however,some bidentate chemical ligands such as OA,sodium carbonate and sodium hydrogen phosphates are even more effective in removing these metals from contaminated water.Furthermore,heavier metals are preferentially removed than lighter metals.
基金supported by the National Natural Science Foundation of China (Nos. 21878221 and 21476166)the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (No. 21621004)。
文摘Oriented ligand immobilization is one of the most effective strategies used in the design and construction of a high-capacity protein A chromatography. In this work, cysteine was introduced as anchoring sites by substituting a specific residue on Helix Ⅰ, Ⅱ, and at C-terminus of antibody binding domain Z from protein A, respectively, to investigate structural evolution and binding behavior of protein A ligands at liquid-solid interfaces. Among the three affinity dextran-coated Fe_(3)O_(4) magnetic nanoparticles(Fe_(3)O_(4)@Dx MNPs), affinity MNPs with the immobilized ligand via N11C on Helix Ⅰ(Fe_(3)O_(4)@Dx-Z_(1) MNPs) had the highest helical content, and MNPs with the immobilized ligand via G29C on Helix Ⅱ(Fe_(3)O_(4)@Dx-Z_(2) MNPs) had the lowest helical content at the same pHs. It was attributed to less electrostatic attraction of ligand to negatively charged surface on Fe_(3)O_(4)@Dx-Z_(1) MNPs because of less positive charged residues on Helix Ⅰ(K6) than Helix Ⅱ(R27/K35). Among the three affinity MNPs, moreover, the highest affinity to immunoglobulin G(IgG) binding was observed on Fe_(3)O_(4)@Dx-Z_(1) MNPs in isothermal titration calorimetry measurement, further validating greater structural integrity of the ligand on Fe_(3)O_(4)@Dx-Z_(1) MNPs. Finally,the study of IgG binding on MNPs and 96-well plates showed that anchoring sites for ligand immobilization had distinct influences on IgG binding and IgG-mediated antigen binding. This work illustrated that anchoring sites of the ligands had a striking significance for the molecular structure of the ligand at liquid-solid interfaces and raised an important implication for the design and optimization of protein A chromatography and protein A-based immunoassay analysis.
基金the financial support of the Training Program of the Major Research Plan of the National Natural Science Foundation of China(92061124)the National Natural Science Foundation of China(21975292,21978331,22068008,and 52101186)+3 种基金the Guangdong Basic and Applied Basic Research Foundation(2021A1515010167 and 2022A1515011196)the Guangzhou Key R&D Program/Plan Unveiled Flagship Project(20220602JBGS02)the Guangzhou Basic and Applied Basic Research Project(202201011449)the Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202220 and FC202216)。
文摘Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported[Au_(25)(PET)_(18)]-nanoclusters with the preservation of the core structure.This procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment,avoiding the reconfiguration or agglomeration of Au_(25)nanoclusters,where the degree of dethiolation can be regulated by the control of duration.This work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution reaction.Consequently,the activity and selectivity towards CO formation in electrochemical CO_(2)reduction reaction of Au_(25)nanoclusters can be promoted.This work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.
基金financially supported by the National Natural Science Foundation of China (Grants Nos.51772338,51972349,91963210 and U1801255).
文摘The design of efficient and robust non-precious metal electrocatalysts towards oxygen evolution reaction(OER)is of great value for developing green energy technologies.The in-situ formed high-valence(oxy)hydroxides species during the reconstruction process of pre-catalysts are recognized as the real contributing sites for OER.However,pre-catalysts generally undergo a slow and inadequate self-reconstruction.Herein,we reported a PO^(3-)_(4)optimized CoFe-based OER catalysts with amorphous structure,which enables a fast and deep reconstruction during the OER process.The amorphous structure induced by ligands PO^(3-)_(4)is prone to evolution and further form active species for OER.The electron interaction between metal sites can be modulated by electron-rich PO^(3-)_(4),which promotes generation of high active CoOOH.Simultaneously,the etching of PO^(3-)_(4)from the pre-catalysts during the catalytic process is in favor of accelerating the self-reconstruction.As a result,as-prepared precatalyst can generate high active CoOOH at a low potential of 1.4 V and achieve an in-depth reconstructed nanosheet structure with abundant OER active sites.Our work provides a promising design of pre-catalysts for realizing efficient catalysis of water oxidation.
基金supported by the National Natural Science Foundation of China(22072034,22001050,and 21873025)the China Postdoctoral Science Foundation(2020T130147,2020M681084,and 2022M710949)+1 种基金the Postdoctoral Foundation of Heilongjiang Province(LBH-Z19059)the Natural Science Foundation of Heilongjiang Youth Fund(YQ2021B002).
文摘Deep-level defects and random oriented configuration in perovskite crystallization process would cause the nonradiative recombination and further affect the performance of perovskite solar cells(PSCs).Herein,two metal-organic frameworks(MOFs)with tunable Lewis-base passivation sites have been constructed(Cd-Httb and Cd-Httb-BDC,Httb=5-(4-(1H-1,2,4-triazole-1-yl)benzyl)-1h-tetrazole,BDC=1,4-dicarboxybenzene)to eliminate deep-level defects and simultaneously as nanostructured heterogeneous nucleation seed to assist the growth of large-grained perovskite films.Compared with the control and Cd-Httb,Cd-Httb-BDC designed with mix-ligands strategy exhibited the enhanced inducted effect on the crystallization and nucleation of high-quality perovskite films during annealing process.Consequently,the resultant Cd-Httb-BDC-modified device achieved higher power conversion efficiency(PCE)(22.18%)than the control(20.89%)and Cd-Httb(21.56%).Meanwhile,the unencapsulated Cd-Httb-BDC-modified device still maintained 90%of initial PCE after 1500 h in ambient conditions and exhibited enhanced thermal stability(85℃ in N_(2) atmosphere).This work presented a successful example of mixligands strategy on construction of high-quality MOF-assisted perovskite films for high-efficient and stable PSCs.
文摘Cancer is one of the most prevalent diseases worldwide,which causes significant morbidity and mortality.Designing and developing a potential anti-cancer drug is an active field of research worldwide.Microorganisms have been considered a potential source of anti-cancer drugs.One such microbe-derived compound is surfactin,which shows potential anti-cancer activities.In this study,we evaluated the binding potential of surfactin with several cancer cell ligands via an in-silico approach.Hence,molecular docking studies were performed to test the binding potential of surfactin against four targets.The analyses revealed that surfactin from Bacillus sp.can bind with the targeted ligands(coenzyme A,D-leucine,glycerol,and(R)-3-hydroxytetradecanal)with significant affinity.Surfactin showed the highest binding affinity(-7.7 kcal mol-1)to coenzyme A among the targeted ligands.These results may be useful for developing anti-cancer drugs.Nevertheless,further experimental studies are needed to investigate the ligand binding capacity and anti-cancer potential of such surfactin-like molecules.
基金supported by National Key Research&Development Program of China (2022YFA1506200)the National Natural Science Foundations of China (22078007, 21627813, 21706009,22002085)+3 种基金Guangdong Basic and Applied Basic Research Foundation (2020A1515110832)the Fundamental Research Funds for the Central Universities (buctrc201921, JD2223)Innovative Achievement Commercialization Service-Platform of Industrial CatalysisChemistry and Chemical Engineering Guangdong Laboratory for a startup funding support(2111001)
文摘Bimetallic nanoparticles exhibit a synergistic effect that critically depends on their surface composition,but such promotion mechanisms become vague with varying surface compositions.Here,alumina supported Ag@Pd core–shell and PdAg alloy structure with controlled size and surface compositions were prepared to demonstrate synergetic mechanisms,particularly,ligand and strain effects on activity and ethylene selectivity for acetylene hydrogenation.The performance evaluation indicates that Ag@Pd catalysts with well-controlled Pd-shell thickness can effectively lower apparent activation energy and improve ethylene selectivity.Hydrogenation activity increases from 0.019 to 0.062 s^(-1) with decreasing Pd-shell thickness under mild conditions,which is 3–6 times higher than their alloyed and monometallic counterparts.Combined characterizations and density functional theory are conducted to reveal such shell-thickness-dependent performance.The ligand effect arising from Ag alloying in the interface of Ag@Pd2ML observes the strongest binding of acetylene,but it diminished sharply and the strain effect gets more prevailing with increasing shell thickness.The competition of ethylene desorption and deephydrogenation were also investigated to understand the selectivity governing factors,and the selectivity descriptor(0.5BE(C_(2)H_(4))–BE(H))was built to match the contribution of ligand and strain effect on the different surfaces of Pd-Ag bimetallic NPs.The exploration of synergetic mechanisms among bimetallic NPs with varied structure and surface compositions in this work can help us to deepen the understanding catalyst structure–activity relationship and provide a feasible way to optimize the overall catalytic performance.
基金supported by the National Natural Science Foundation of China(61935016,62275213 and 62205264),the National Natural Science Foundation of China(21961160720)the Fundamental Research Funds for Xi'an Jiaotong University(xzy012022092,xzd012022003 and xzy022022057)+1 种基金the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)。
文摘Perovskite solar cells(PSCs)have attracted aggressive attention in the photovoltaic field in light of the rapid increasing power conversion efficiency.However,their large-scale application and commercialization are limited by the toxicity issue of lead(Pb).Among all the lead-free perovskites,tin(Sn)-based perovskites have shown potential due to their low toxicity,ideal bandgap structure,high carrier mobility,and long hot carrier lifetime.Great progress of Sn-based PSCs has been realized in recent years,and the certified efficiency has now reached over 14%.Nevertheless,this record still falls far behind the theoretical calculations.This is likely due to the uncontrolled nucleation states and pronounced Sn(Ⅳ)vacancies.With insights into the methodologies resolving both issues,ligand engineering-assisted perovskite film fabrication dictates the state-of-the-art Sn-based PSCs.Herein,we summarize the role of ligand engineering during each state of film fabrication,ranging from the starting precursors to the ending fabricated bulks.The incorporation of ligands to suppress Sn~(2+)oxidation,passivate bulk defects,optimize crystal orientation,and improve stability is discussed,respectively.Finally,the remained challenges and perspectives toward advancing the performance of Sn-based PSCs are presented.We expect this review can draw a clear roadmap to facilitate Sn-based PSCs via ligand engineering.
基金supported by the National Key Research and Development Program of China(Nos.2021YFB3602703,2022YFB3606504,and 2022YFB3602903)National Natural Science Foundation of China(No.62122034)+3 种基金Guangdong University Key Laboratory for Advanced Quantum Dot Displays and Lighting(No.2017KSYS007)Shenzhen Key Laboratory for Advanced Quantum Dot Displays and Lighting(No.ZDSYS201707281632549)Shenzhen Science and Technology Program(No.JCYJ20220818100411025)Shenzhen Development and Reform Commission Project(No.XMHT20220114005)。
文摘The performance of inverted quantum-dot light-emitting diodes(QLEDs)based on solution-processed hole transport layers(HTLs)has been limited by the solvent-induced damage to the quantum dot(QD)layer during the spin-coating of the HTL.The lack of compatibility between the HTL’s solvent and the QD layer results in an uneven surface,which negatively impacts the overall device performance.In this work,we develop a novel method to solve this problem by modifying the QD film with 1,8-diaminooctane to improve the resistance of the QD layer for the HTL’s solvent.The uniform QD layer leads the inverted red QLED device to achieve a low turn-on voltage of 1.8 V,a high maximum luminance of 105500 cd/m2,and a remarkable maximum external quantum efficiency of 13.34%.This approach releases the considerable potential of HTL materials selection and offers a promising avenue for the development of high-performance inverted QLEDs.
基金supported by the National Natural Science Foundation of China,Nos. 82071304 (to QXZ), 81671149 (to QXZ),and 81971179 (to XML)the Natural Science Foundation of Jiangsu Province,Nos. BK20191463 (to XML) and BK20161167 (to QXZ)。
文摘We previously reported that postsynaptic density-93 mediates neuron-microglia crosstalk by interacting with amino acids 357–395 of C-X3-C motif chemokine ligand 1(CX3 CL1) to induce microglia polarization. More importantly, the peptide Tat-CX3 CL1(comprising amino acids 357–395 of CX3 CL1) disrupts the interaction between postsynaptic density-93 and CX3 CL1, reducing neurological impairment and exerting a protective effect in the context of acute ischemic stroke. However, the mechanism underlying these effects remains unclear. In the current study, we found that the pro-inflammatory M1 phenotype increased and the anti-inflammatory M2 phenotype decreased at different time points. The M1 phenotype increased at 6 hours after stroke and peaked at 24 hours after perfusion, whereas the M2 phenotype decreased at 6 and 24 hours following reperfusion. We found that the peptide Tat-CX3 CL1(357–395 aa) facilitates microglial polarization from M1 to M2 by reducing the production of soluble CX3 CL1. Furthermore, the a disintegrin and metalloprotease domain 17(ADAM17) inhibitor GW280264 x, which inhibits metalloprotease activity and prevents CX3 CL1 from being sheared into its soluble form, facilitated microglial polarization from M1 to M2 by inhibiting soluble CX3 CL1 formation. Additionally, Tat-CX3 CL1(357–395 aa) attenuated long-term cognitive deficits and improved white matter integrity as determined by the Morris water maze test at 31–34 days following surgery and immunofluorescence staining at 35 days after stroke, respectively. In conclusion, Tat-CX3 CL1(357–395 aa) facilitates functional recovery after ischemic stroke by promoting microglial polarization from M1 to M2. Therefore, the Tat-CX3 CL1(357–395 aa) is a potential therapeutic agent for ischemic stroke.
